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首页> 外文期刊>Journal of the American Chemical Society >Uniform Biodegradable Fiber-Like Micelles and Block Comicelles via 'Living' Crystallization-Driven Self-Assembly of Poly(L-lactide) Block Copolymers: The Importance of Reducing Unimer Self-Nucleation via Hydrogen Bond Disruption
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Uniform Biodegradable Fiber-Like Micelles and Block Comicelles via 'Living' Crystallization-Driven Self-Assembly of Poly(L-lactide) Block Copolymers: The Importance of Reducing Unimer Self-Nucleation via Hydrogen Bond Disruption

机译：聚（L-丙交酯）嵌段共聚物通过“活性”结晶驱动的自组装形成均匀的可生物降解的纤维状胶束和胶束：通过氢键断裂减少单体自成核的重要性

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Fiber-like micelles based on biodegradable and biocompatible polymers exhibit considerable promise for applications in nanomedicine, but until recently no convenient methods were available to prepare samples with uniform and controllable dimensions and spatial control of functionality. “Living” crystallization-driven self-assembly (CDSA) is a seeded growth method of growing importance for the preparation of uniform 1D and 2D core–shell nanoparticles from a range of crystallizable polymeric amphiphiles. However, in the case of poly(l-lactide) (PLLA), arguably the most widely utilized biodegradable polymer as the crystallizable core-forming block, the controlled formation of uniform fiber-like structures over a substantial range of lengths by “living” CDSA has been a major challenge. Herein, we demonstrate that via simple modulation of the solvent conditions via the addition of trifluoroethanol (TFE), DMSO, DMF and acetone, uniform fiber-like nanoparticles from PLLA diblock copolymers with controlled lengths up to 1 μm can be prepared. The probable mechanism involves improved unimer solvation by a reduction of hydrogen bonding interactions among PLLA chains. We provide evidence that this minimizes undesirable unimer aggregation which otherwise favors self-nucleation that competes with epitaxial crystallization from seed termini. This approach has also allowed the formation of well-defined segmented block comicelles with PLLA cores via the sequential seeded-growth of PLLA block copolymers with different corona-forming blocks.
机译：基于可生物降解和生物相容性聚合物的纤维状胶束在纳米医学中具有广阔的应用前景，但直到最近，还没有便捷的方法可用于制备具有均一且可控的尺寸以及功能性空间控制的样品。 “活的”结晶驱动自组装（CDSA）是一种种子生长方法，对于从一系列可结晶的聚合物两亲物中制备均匀的1D和2D核-壳纳米粒子，其重要性日益提高。但是，就聚（l-丙交酯）（PLLA）而言，可以说是最广泛使用的可生物降解的聚合物作为可结晶的核形成嵌段，通过“活着”在相当长的长度范围内可控地形成均匀的纤维状结构CDSA是一个重大挑战。在此，我们证明，通过添加三氟乙醇（TFE），DMSO，DMF和丙酮，通过简单地调节溶剂条件，可以制得PLLA二嵌段共聚物，其长度可控制至1μm的均匀纤维状纳米颗粒。可能的机制包括通过降低PLLA链之间的氢键相互作用来改善单体聚合。我们提供的证据表明，这可最大程度地减少不良的单体聚合，否则单体聚合会促进自成核，从而与种子末端的外延结晶竞争。这种方法还允许通过具有不同电晕形成嵌段的PLLA嵌段共聚物的连续种子生长，形成带有PLLA核的明确定义的嵌段嵌段共聚物。

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